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At the French Open, Suárez Navarro reached the quarterfinals of her first Grand Slam main draw tournament. After she won three qualifying matches, she defeated former world No. 1 Amélie Mauresmo of France in the second round 6–3, 6–4, Australian Casey Dellacqua in the third round, and 26th-seeded Italian Flavia Pennetta in the fourth round 6–3, 6–2. Suárez Navarro then lost to third-seeded Jelena Janković in the quarterfinals 3–6, 2–6. At Wimbledon, she lost to second-seeded Janković in the second round 1–6, 3–6.

At Wimbledon, Suárez Navarro defeated No. 25 Kaia Kanepi in the first round and Ekaterina Makarova in the second. She faced defending champion Venus Williams for the first time since the 2009 Australian Open but was unable to repeat the upset win, losing 0–6, 4–6.

Suárez Navarro had a good start to 2010, making the second round of the ASB Classic in Auckland before losing to top seed Flavia Pennetta in straight sets. She then made the quarterfinal of the Hobart International before losing to No. 2 seed Shahar Pe'er 6–4, 6–7, 5–7.

At the Australian Open, Suárez Navarro made it to the third round before losing to top seed, the defending (and eventual) champion Serena Williams, 0–6, 3–6.

Unseeded at the BNP Paribas Open at Indian Wells, California, Suárez Navarro reached the fourth round, losing to Alisa Kleybanova 6–2, 6–7, 4–6. Along the way, she gained one of the biggest wins of her career by defeating world No. 3 and top seed Svetlana Kuznetsova, 6–4, 4–6, 6–1 in the second round.

She reached the final of the Andalucia Tennis Experience in Marbella for the second year in a row, losing to Flavia Pennetta 2–6, 6–4, 3–6.

Suarez Navarro suffered an ankle injury at the tournament in Fes, Morocco. She returned to play in the French Open, losing her first-round match to Olga Govortsova 6–7, 1–6, she remained sidelined until the US Open.

Then, Suárez followed an early loss in Paris with a semifinal and a quarterfinal, in Bogotá and Acapulco, respectively. An elbow injury caused her to stop playing for two and a half months and withdraw from Roland Garros.

At the French Open she was seeded eighth. She lost to Jelena Ostapenko in the first round of Wimbledon that year, and her results for the rest of the year were inauspicious apart from reaching the quarterfinals in Moscow in October and a crushing 6–0, 6–0 victory over an injured Andrea Petkovic at Zhuhai in November. Carla ended the year ranked 13th.

Suárez Navarro made a good start to the year. She reached the semifinals at Brisbane, losing to Angelique Kerber, and the quarterfinals of the Australian Open, losing to Agnieszka Radwańska. As a result, she moved back up to world No. 8 on February 1. She then defeated Jelena Janković in Spain's Fed Cup tie against Serbia.

At the Dubai Tennis Championships, she received a first round bye but fell to eventual semifinalist Caroline Garcia. Her next tournament was the Qatar Open where she also received a first-round bye and defeated Donna Vekić, Timea Bacsinszky, Elena Vesnina and Agnieszka Radwańska en route to the final, ensuring a new career-high ranking of world No. 6. She then avenged her first round loss to Jelena Ostapenko in the previous year's Wimbledon with a three set win over Ostapenko, earning her first Premier title and her biggest title to date.

Suárez Navarro uses a single-handed backhand, unlike most female players of her era.[5] She has said in interviews that her favorite shot is her cross-court backhand and that her favourite surfaces are clay and hard. Frew McMillan has said, "There's something of Justine Henin about her game. She has a great variety of shots."[6]